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Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries

Author

Listed:
  • Yingqi Liu

    (Tsinghua University)

  • Zhiyuan Zhang

    (Tsinghua University)

  • Junyang Tan

    (Tsinghua University)

  • Biao Chen

    (Tianjin University)

  • Bingyi Lu

    (Tsinghua University)

  • Rui Mao

    (Tsinghua University)

  • Bilu Liu

    (Tsinghua University)

  • Dashuai Wang

    (Zhejiang University)

  • Guangmin Zhou

    (Tsinghua University)

  • Hui-Ming Cheng

    (Chinese Academy of Sciences
    Chinese Academy of Sciences
    Shenzhen University of Advanced Technology)

Abstract

Developing highly efficient catalysts is significant for Li-CO2 batteries. However, understanding the exact structure of catalysts during battery operation remains a challenge, which hampers knowledge-driven optimization. Here we use X-ray absorption spectroscopy to probe the reconstruction of CoSx (x = 8/9, 1.097, and 2) pre-catalysts and identify the local geometric ligand environment of cobalt during cycling in the Li-CO2 batteries. We find that different oxidized states after reconstruction are decisive to battery performance. Specifically, complete oxidation on CoS1.097 and Co9S8 leads to electrochemical performance deterioration, while oxidation on CoS2 terminates with Co-S4-O2 motifs, leading to improved activity. Density functional theory calculations show that partial oxidation contributes to charge redistributions on cobalt and thus facilitates the catalytic ability. Together, the spectroscopic and electrochemical results provide valuable insight into the structural evolution during cycling and the structure-activity relationship in the electrocatalyst study of Li-CO2 batteries.

Suggested Citation

  • Yingqi Liu & Zhiyuan Zhang & Junyang Tan & Biao Chen & Bingyi Lu & Rui Mao & Bilu Liu & Dashuai Wang & Guangmin Zhou & Hui-Ming Cheng, 2024. "Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46465-8
    DOI: 10.1038/s41467-024-46465-8
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    References listed on IDEAS

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    1. Deqing Cao & Chuan Tan & Yuhui Chen, 2022. "Oxidative decomposition mechanisms of lithium carbonate on carbon substrates in lithium battery chemistries," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    2. Duo Wei & Rui Sang & Peter Sponholz & Henrik Junge & Matthias Beller, 2022. "Reversible hydrogenation of carbon dioxide to formic acid using a Mn-pincer complex in the presence of lysine," Nature Energy, Nature, vol. 7(5), pages 438-447, May.
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